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The method for assigning an object's values to an array of objects by using the key would involve iterating through the object and accessing each key-value pair. Then, for each key-value pair, a new object would be created with a matching key and the corresponding value, and that new object would be added to the array. Here is an example in JavaScript:

const myObj = {
  name: "John",
  age: 28,
  gender: "male"
};

const myArr = [];

for (const key in myObj) {
  const newObj = {
    key: key,
    value: myObj[key]
  };
  myArr.push(newObj);
}

console.log(myArr); // [{ key: "name", value: "John" }, { key: "age", value: 28 }, { key: "gender", value: "male" }]

In this example, we start with an object myObj with three key-value pairs. We then iterate through the object using a for...in loop, creating a new object for each key-value pair with a key property set to the current key and a value property set to the current value. Each new object is then added to the myArr array using the push() method. Finally, we log out the resulting array of objects.